CAREER: Theoretical Analysis of Molecular Oxygen Chemistry in Biological Systems

威斯康星大学的崔强通过一个职业奖项得到了理论和计算化学项目的支持，该项目旨在开发和应用混合量子力学/分子力学方法来探索黄素-氧化学在黄素蛋白质中的细节。具体地说，约束密度泛函理论将被用来构造与黄素和分子氧之间的电子转移相关的非绝热状态。用系综平均密度泛函理论平衡地描述了黄素-超氧自由基对自旋禁戒跃迁的三重态和单态电子态。这些方法可以扩展到与其他涉及分子氧的化学过程有关的能量学和动力学性质。此外，还将为计算生物物理学课程开发完全互动的多媒体材料，以及具有重要教学价值的经典研究论文的网络数据库。理论分析在确定详细的机制和洞察蛋白质活性部位环境的结构和动力学特性方面非常有价值，特别是在仅靠实验无法得出结论的情况下。这项研究项目将扩大酶模拟的范围和详细程度，超越传统的计算方法。此外，新的多媒体教材和基于网络的数据库将平衡现代发展和基本概念，改善学生的学习体验。

Qiang Cui of the University of Wisconsin is supported by the Theoretical and Computational Chemistry Program through a CAREER award to develop and apply hybrid quantum mechanical/molecular mechanical methods to explore details of flavin-oxygen chemistry in flavoproteins. Specifically, a constrained density functional theory will be used to construct diabatic states relevant to electron transfer between flavin and molecular oxygen. Ensemble-averaged density functional theory will be used to achieve a balanced description of both triplet and singlet electronic states of the flavin-superoxide radical pair undergoing a spin-forbidden transition. These methods can be extended to the energetics and kinetic properties associated with other chemical processes involving molecular oxygen. In addition, fully interactive, multimedia material will be developed for computational biophysics courses, along with a web-based database of classic research papers with great pedagogical value.Theoretical analysis is very valuable in identifying detailed mechanisms and providing insights into the structural and dynamical properites of protein active site environments, especially when experiments alone are inconclusive. This research project will expand the scope and level of detail for enzyme simulations beyond what conventional computational methods offer. In addition, new multimedia course material and a web-based database will improve the student learning experience by incorporating a balance of modern developments and fundamental concepts.